Highly Stable and Minimally Pt-Loaded Multiporous Bimetallic Matryoshka Heterostructures for Efficient Hydrogen Evolution Reaction via pH-Dependent Mechanistic Decoupling Dun Chan Cha, Sumin Kim, Hyun Seung Lee, Seong Chan Cho, Hayoung Kim, et al. Advanced Synthesis and Catalysis, 2026 Developing highly efficient and stable electrocatalysts with minimized platinum (Pt) loading is critical for sustainable hydrogen production via water splitting. However, optimizing performance across a wide pH range remains challenging due to distinct reaction mechanisms and stability issues, particularly in corrosive acidic environments. Herein, we report the synthesis of highly uniform and porous Au–Pt Matryoshka heterostructures via a facile galvanic replacement reaction using Au nanorods as templates. This unique architecture maximizes atomic utilization while maintaining a low Pt content in the optimized Pt‐Matryoshka catalysts. Our results indicate distinct pH‐dependent differences in the dominant factors governing the hydrogen evolution reaction activity. In alkaline media (1 M KOH), the activity was dominantly governed by the electrochemically active surface area (ECSA), where the Pt‐100 catalyst exhibited the highest ECSA and a low overpotential of 129 mV at 10 mA cm −2 . Conversely, in acidic media (0.1 M H 2 SO 4 ), the activity was closely associated with charge–transfer kinetics and catalytic properties, rather than being solely governed by surface area effects. The optimized Pt‐150 catalyst achieved an ultra‐low overpotential of 62 mV, comparable to commercial 10% Pt/C, with an exceptionally low Tafel slope of 23 mV dec −1 , indicating a shift to the rapid Volmer–Tafel mechanism. Notably, the Pt‐Matryoshka structure demonstrated excellent durability in highly corrosive acidic conditions, showing a negligible potential degradation of only 0.012 V after 60 h of operation. This improved stability is associated with the synergistic effect of the Au–Pt alloy interface, which suggests limited metal dissolution. This study provides critical insights into the decoupling of pH‐dependent performance factors and presents a robust strategy for designing durable, low‐Pt electrocatalysts for broad‐range pH applications.
Synchronization of Emerging Materials and their Synthetic Strategies for Efficient Alkaline Water Splitting Dun Chan Cha, Chandan Kumar, Ashakiran Maibam, Sunghoon Yoo, Jaejun Park, et al. Chemelectrochem, 2025 Hydrogen is considered the “future fuel” due to its zero‐carbon emissions, high gravimetric energy density, and sustainability. However, the generation of hydrogen through the splitting of water requires highly efficient bifunctional electrocatalysts to overcome the sluggish kinetics of each half‐cell reaction, the oxygen evolution reaction (OER) at the anode and the hydrogen evolution reaction (HER) at the cathode. Various emerging materials, including metal‐organic frameworks, 2D materials, single‐atom catalysts, high‐entropy alloys, perovskites, and MXenes, have shown great potential for OER and HER. However, the synthesis strategies for these materials vary significantly based on their unique physicochemical properties. There has been no proper study on synthesis strategies for each class of the emerging materials or synchronization of the heterostructures formed. The variety in emerging materials and available synthesis routes presents ample opportunity for further exploration of target‐oriented materials with unique properties. This review covers recent advancement of emerging materials and their synchronization with existing synthesis strategies for high electrocatalytic activities in water splitting. The review further discusses the challenges and future opportunities for utilizing such emerging materials in water splitting.
Tunable B-Doped Cobalt Phosphide Nanosheets Engineered via Phosphorus Activation of Co-MOFs for High Efficiency Alkaline Water-Splitting Dun Chan Cha, Jun Ho Seok, Seong Chan Cho, Manjinder Singh, Thangjam Ibomcha Singh, et al. Small, 2025 Introducing secondary heteroatoms and simultaneous in situ surface modification can enhance electrocatalysts by affecting their porosity for adjusting electrochemically active surface area (ECSA), number of active sites, and electronic properties, thus mitigating the sluggish kinetics of oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in alkaline media. Here, mesoporous 3D heterostructures of boron‐doped cobalt phosphide@nitrogen‐doped carbon nanosheet network arrays are successfully grown on Ni foam as free‐standing bifunctional electrocatalysts with controlled phosphorous levels (B‐CoPx@NC/NF, x = 0.25, 0.5, and 1). Boron doping induces the Co active sites to bind O* and OOH* intermediates. Meanwhile, an optimal phosphorous content also leads to ideal adsorption strength at each reaction step, satisfying the Sabatier principle well. The optimal B‐CoP0.5@NC/NF requires low overpotentials of 248 mV for OER and 95 mV for HER with long‐term stability. The B‐CoP0.5@NC/NF (+/−) electrolyzer exhibits a low cell potential of 1.59 V at 10 mA cm−2 for overall water‐splitting, with superior activity compared to the RuO2/NF(+)//20%Pt/NF(−) electrolyzer at high current densities above 50 mA cm−2. Such exceptional bifunctional activities are attributed to the modulated electronic structure, lower charge‐transfer resistance, higher ECSA, and inductive effect of B‐doping, thus boosting both OER and HER activities in alkaline media.
A critical review on amorphous-crystalline heterostructured electrocatalysts for efficient water splitting Manjinder Singh, Dun Chan Cha, Thangjam Ibomcha Singh, Ashakiran Maibam, Dasu Ram Paudel, et al. Materials Chemistry Frontiers, 2023 This review presents comprehensive details on recent developments in the fabrication of different amorphous–crystalline heterostructures, their compositions, and the resulting physicochemical properties for OER, HER, and overall water splitting.
Free-standing bi-metal organic-framework-derived Zn-Co oxide bifunctional electrocatalyst for electrocatalytic alkaline water splitting SS Heikrujam, SJ Chanu, SB Singh, H Jeong, TI Singh, KN Devi Applied Surface Science, 167243 , 2026 2026
Highly Stable and Minimally Pt‐Loaded Multiporous Bimetallic Matryoshka Heterostructures for Efficient Hydrogen Evolution Reaction via pH‐Dependent Mechanistic Decoupling DC Cha, S Kim, HS Lee, SC Cho, H Kim, TI Singh, SJ Min, SU Lee, S Lee Advanced Synthesis & Catalysis 368 (9), e70491 , 2026 2026
MOF-derived ZnO/CuO nanocomposite for efficient degradation of Imidacloprid and Its Degradation Pathway Evaluation LA Chanu, S Phanjoubam, KJ Singh, TI Singh, AS Koijam, HN Sharma, ... Materials Chemistry and Physics, 132047 , 2026 2026
Water electrolysis catalyst with core-shell structure and method for preparing same S Lee, TI SINGH, DC CHA, S KIM US Patent 12,404,594 , 2025 2025
Front Cover: Synchronization of Emerging Materials and their Synthetic Strategies for Efficient Alkaline Water Splitting (ChemElectroChem 17/2025) DC Cha, C Kumar, A Maibam, S Yoo, J Park, S Kim, H Kim, TI Singh, ... ChemElectroChem 12 (17), e70032 , 2025 2025
Synchronization of Emerging Materials and their Synthetic Strategies for Efficient Alkaline Water Splitting DC Cha, C Kumar, A Maibam, S Yoo, J Park, S Kim, H Kim, TI Singh, ... ChemElectroChem 12 (17), e202500014 , 2025 2025 Citations: 4
Tunable B‐Doped Cobalt Phosphide Nanosheets Engineered via Phosphorus Activation of Co‐MOFs for High Efficiency Alkaline Water‐Splitting DC Cha, JH Seok, SC Cho, M Singh, TI Singh, SU Lee, S Lee Small 21 (31), 2500334 , 2025 2025 Citations: 29
Cobalt substitution on SnS-rGO composites for efficient oxygen and hydrogen evolution reactions C Kumar, P Saharan, TI Singh, A Gupta, J Singh, M Singh, SR Dhakate Energy & Fuels 38 (17), 16861-16872 , 2024 2024 Citations: 6
Tailoring tin sulfide electrocatalyst with petroleum coke derived reduced graphene oxide for overall water splitting C Kumar, TI Singh, P Saharan, A Gupta, J Singh, M Singh, SR Dhakate FlatChem 46, 100689 , 2024 2024 Citations: 5
Achieving the optimal performance of VO@ CoNC anchored on MX/CF through phosphorous-doped induced defects for the fiber-shaped solid-state Zn-ion battery DD Khumujam, T Kshetri, TI Singh, SB Singh, NH Kim, JH Lee Chemical Engineering Journal 486, 150252 , 2024 2024 Citations: 18
Counter ion-regulated heterostructured Co@ Fe-based core@ shell materials: as remarkable bifunctional electrodes for green H 2 production G Rajeshkhanna, A Borah, TI Singh, TH Nguyen, VA Dinh, NH Kim, ... Journal of Materials Chemistry A 12 (36), 24656-24669 , 2024 2024 Citations: 13
Hierarchical integrated hybrid structural electrodes based on Co‐N/C and Mo‐doped NiCo‐LDH@ Co‐N/C anchored on MX/CF for high energy density fiber‐shaped supercapacitor DD Khumujam, T Kshetri, TI Singh, NH Kim, JH Lee Advanced Functional Materials 33 (40), 2302388 , 2023 2023 Citations: 77
Metal–Organic Framework–Derived Mesoporous B‐Doped CoO/Co@ N‐Doped Carbon Hybrid 3D Heterostructured Interfaces with Modulated Cobalt Oxidation States for Alkaline Water … DC Cha, TI Singh, A Maibam, TH Kim, DH Nam, R Babarao, S Lee Small 19 (35), 2370283 , 2023 2023 Citations: 1
Metal–organic framework–derived mesoporous B‐doped CoO/Co@ N‐doped carbon hybrid 3D heterostructured interfaces with modulated cobalt oxidation states for alkaline water splitting DC Cha, TI Singh, A Maibam, TH Kim, DH Nam, R Babarao, S Lee Small 19 (35), 2301405 , 2023 2023 Citations: 62
Photocatalytic Hydrogen Production by Biomass Reforming TI Singh, S Li, G Leem, S Lee Photocatalytic Hydrogen Production for Sustainable Energy, 191-217 , 2023 2023 Citations: 3
A critical review on amorphous–crystalline heterostructured electrocatalysts for efficient water splitting M Singh, DC Cha, TI Singh, A Maibam, DR Paudel, DH Nam, TH Kim, ... Materials Chemistry Frontiers 7 (24), 6254-6280 , 2023 2023 Citations: 64
Fibrous asymmetric supercapacitor based on wet spun MXene/PAN Fiber-derived multichannel porous MXene/CF negatrode and NiCo2S4 electrodeposited MXene/CF positrode DD Khumujam, T Kshetri, TI Singh, NH Kim, JH Lee Chemical Engineering Journal 449, 137732 , 2022 2022 Citations: 99
High‐Alkaline Water‐Splitting Activity of Mesoporous 3D Heterostructures: An Amorphous‐Shell@ Crystalline‐Core Nano‐Assembly of Co‐Ni‐Phosphate Ultrathin‐Nanosheets and V‐Doped … TI Singh, A Maibam, DC Cha, S Yoo, R Babarao, SU Lee, S Lee Advanced Science 9 (23), 2270141 , 2022 2022 Citations: 1
High‐alkaline water‐splitting activity of mesoporous 3D heterostructures: an amorphous‐shell@ crystalline‐core nano‐assembly of Co‐Ni‐phosphate ultrathin‐nanosheets and V‐doped … TI Singh, A Maibam, DC Cha, S Yoo, R Babarao, SU Lee, S Lee Advanced Science 9 (23), 2201311 , 2022 2022 Citations: 128
Co-MOF@ MXene-carbon nanofiber-based freestanding electrodes for a flexible and wearable quasi-solid-state supercapacitor T Kshetri, DD Khumujam, TI Singh, YS Lee, NH Kim, JH Lee Chemical Engineering Journal 437, 135338 , 2022 2022 Citations: 178
MOST CITED SCHOLAR PUBLICATIONS
Alkaline water splitting enhancement by MOF‐derived Fe–Co–oxide/Co@ NC‐mNS heterostructure: boosting OER and HER through defect engineering and in situ oxidation TI Singh, G Rajeshkhanna, UN Pan, T Kshetri, H Lin, NH Kim, JH Lee Small 17 (29), 2101312 , 2021 2021 Citations: 312
Co-MOF@ MXene-carbon nanofiber-based freestanding electrodes for a flexible and wearable quasi-solid-state supercapacitor T Kshetri, DD Khumujam, TI Singh, YS Lee, NH Kim, JH Lee Chemical Engineering Journal 437, 135338 , 2022 2022 Citations: 178
Remarkable bifunctional oxygen and hydrogen evolution electrocatalytic activities with trace-level Fe doping in Ni-and Co-layered double hydroxides for overall water-splitting G Rajeshkhanna, TI Singh, NH Kim, JH Lee ACS Applied Materials & Interfaces 10 (49), 42453-42468 , 2018 2018 Citations: 167
High‐alkaline water‐splitting activity of mesoporous 3D heterostructures: an amorphous‐shell@ crystalline‐core nano‐assembly of Co‐Ni‐phosphate ultrathin‐nanosheets and V‐doped … TI Singh, A Maibam, DC Cha, S Yoo, R Babarao, SU Lee, S Lee Advanced Science 9 (23), 2201311 , 2022 2022 Citations: 128
Fe and P doped 1T-phase enriched WS23D-dendritic nanostructures for efficient overall water splitting DR Paudel, UN Pan, TI Singh, CC Gudal, NH Kim, JH Lee Applied Catalysis B: Environmental 286, 119897 , 2021 2021 Citations: 127
Flexible transparent supercapacitor with core-shell Cu@ Ni@ NiCoS nanofibers network electrode BS Soram, IS Thangjam, JY Dai, T Kshetri, NH Kim, JH Lee Chemical Engineering Journal 395, 125019 , 2020 2020 Citations: 125
A core–shell MnO 2@ Au nanofiber network as a high-performance flexible transparent supercapacitor electrode SB Singh, TI Singh, NH Kim, JH Lee Journal of Materials Chemistry A 7 (17), 10672-10683 , 2019 2019 Citations: 113
Embedded PEDOT: PSS/AgNFs network flexible transparent electrode for solid-state supercapacitor SB Singh, T Kshetri, TI Singh, NH Kim, JH Lee Chemical Engineering Journal 359, 197-207 , 2019 2019 Citations: 107
Metal organic framework-derived cobalt telluride-carbon porous structured composites for high-performance supercapacitor T Kshetri, TI Singh, YS Lee, DD Khumujam, NH Kim, JH Lee Composites Part B: Engineering 211, 108624 , 2021 2021 Citations: 100
Fibrous asymmetric supercapacitor based on wet spun MXene/PAN Fiber-derived multichannel porous MXene/CF negatrode and NiCo2S4 electrodeposited MXene/CF positrode DD Khumujam, T Kshetri, TI Singh, NH Kim, JH Lee Chemical Engineering Journal 449, 137732 , 2022 2022 Citations: 99
Metal–Organic Framework‐Derived Fe/Co‐based Bifunctional Electrode for H 2 Production through Water and Urea Electrolysis TI Singh, G Rajeshkhanna, SB Singh, T Kshetri, NH Kim, JH Lee ChemSusChem 12 (21), 4810-4823 , 2019 2019 Citations: 92
High-performance solid-state hybrid supercapacitor enabled by metal–organic framework-derived multi-component hybrid electrodes of Co–N–C nanofibers and Co 2− x Fe x P–N–C … TI Singh, G Rajeshkhanna, T Kshetri, NH Kim, JH Lee Journal of Materials Chemistry A 8 (48), 26158-26174 , 2020 2020 Citations: 79
Hierarchical integrated hybrid structural electrodes based on Co‐N/C and Mo‐doped NiCo‐LDH@ Co‐N/C anchored on MX/CF for high energy density fiber‐shaped supercapacitor DD Khumujam, T Kshetri, TI Singh, NH Kim, JH Lee Advanced Functional Materials 33 (40), 2302388 , 2023 2023 Citations: 77
Covalent doping of Ni and P on 1T-enriched MoS 2 bifunctional 2D-nanostructures with active basal planes and expanded interlayers boosts electrocatalytic water splitting UN Pan, TI Singh, DR Paudel, CC Gudal, NH Kim, JH Lee Journal of Materials Chemistry A 8 (37), 19654-19664 , 2020 2020 Citations: 70
Ni-nanoclusters hybridized 1T–Mn–VTe2 mesoporous nanosheets for ultra-low potential water splitting UN Pan, DR Paudel, AK Das, TI Singh, NH Kim, JH Lee Applied Catalysis B: Environmental 301, 120780 , 2022 2022 Citations: 67
A critical review on amorphous–crystalline heterostructured electrocatalysts for efficient water splitting M Singh, DC Cha, TI Singh, A Maibam, DR Paudel, DH Nam, TH Kim, ... Materials Chemistry Frontiers 7 (24), 6254-6280 , 2023 2023 Citations: 64
Metal–organic framework–derived mesoporous B‐doped CoO/Co@ N‐doped carbon hybrid 3D heterostructured interfaces with modulated cobalt oxidation states for alkaline water splitting DC Cha, TI Singh, A Maibam, TH Kim, DH Nam, R Babarao, S Lee Small 19 (35), 2301405 , 2023 2023 Citations: 62
Freestanding 1T‐Mn x Mo 1– x S 2– y Se y and MoFe 2 S 4– z Se z Ultrathin Nanosheet‐Structured Electrodes for Highly Efficient Flexible Solid‐State … UN Pan, V Sharma, T Kshetri, TI Singh, DR Paudel, NH Kim, JH Lee Small 16 (23), 2001691 , 2020 2020 Citations: 59
Mesoporous iron sulfide nanoparticles anchored graphene sheet as an efficient and durable catalyst for oxygen reduction reaction J Gautam, DT Tran, TI Singh, NH Kim, JH Lee Journal of Power Sources 427, 91-100 , 2019 2019 Citations: 58
Effect of reducing agents on the synthesis of anisotropic gold nanoparticles SL Sunghoon Yoo, Dong Hwan Nam, Thangjam Ibomcha Singh, Gyu Leem Nano Convergence 9 (5) , 2022 2022 Citations: 53